TY - JOUR
T1 - Bimetallic Ag-Pt Sub-nanometer Supported Clusters as Highly Efficient and Robust Oxidation Catalysts
AU - Negreiros, Fabio R.
AU - Halder, Avik
AU - Yin, Chunrong
AU - Singh, Akansha
AU - Barcaro, Giovanni
AU - Sementa, Luca
AU - Tyo, Eric C.
AU - Pellin, Michael J.
AU - Bartling, Stephan
AU - Meiwes-Broer, Karl Heinz
AU - Seifert, Sönke
AU - Sen, Prasenjit
AU - Nigam, Sandeep
AU - Majumder, Chiranjib
AU - Fukui, Nobuyuki
AU - Yasumatsu, Hisato
AU - Vajda, Stefan
AU - Fortunelli, Alessandro
N1 - Publisher Copyright:
© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
PY - 2018/1/26
Y1 - 2018/1/26
N2 - A combined experimental and theoretical investigation of Ag-Pt sub-nanometer clusters as heterogeneous catalysts in the CO→CO2 reaction (COox) is presented. Ag9Pt2 and Ag9Pt3 clusters are size-selected in the gas phase, deposited on an ultrathin amorphous alumina support, and tested as catalysts experimentally under realistic conditions and by first-principles simulations at realistic coverage. In situ GISAXS/TPRx demonstrates that the clusters do not sinter or deactivate even after prolonged exposure to reactants at high temperature, and present comparable, extremely high COox catalytic efficiency. Such high activity and stability are ascribed to a synergic role of Ag and Pt in ultranano-aggregates, in which Pt anchors the clusters to the support and binds and activates two CO molecules, while Ag binds and activates O2, and Ag/Pt surface proximity disfavors poisoning by CO or oxidized species.
AB - A combined experimental and theoretical investigation of Ag-Pt sub-nanometer clusters as heterogeneous catalysts in the CO→CO2 reaction (COox) is presented. Ag9Pt2 and Ag9Pt3 clusters are size-selected in the gas phase, deposited on an ultrathin amorphous alumina support, and tested as catalysts experimentally under realistic conditions and by first-principles simulations at realistic coverage. In situ GISAXS/TPRx demonstrates that the clusters do not sinter or deactivate even after prolonged exposure to reactants at high temperature, and present comparable, extremely high COox catalytic efficiency. Such high activity and stability are ascribed to a synergic role of Ag and Pt in ultranano-aggregates, in which Pt anchors the clusters to the support and binds and activates two CO molecules, while Ag binds and activates O2, and Ag/Pt surface proximity disfavors poisoning by CO or oxidized species.
KW - ab initio calculations
KW - alloys
KW - reaction mechanisms
KW - supported catalysts
KW - ultrathin oxide films
UR - http://www.scopus.com/inward/record.url?scp=85039733860&partnerID=8YFLogxK
U2 - 10.1002/anie.201709784
DO - 10.1002/anie.201709784
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C2 - 29239093
AN - SCOPUS:85039733860
SN - 1433-7851
VL - 57
SP - 1209
EP - 1213
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 5
ER -